CN111164800A - Electrode plate, electrode assembly and energy storage device - Google Patents

Electrode plate, electrode assembly and energy storage device Download PDF

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Publication number
CN111164800A
CN111164800A CN201880062760.1A CN201880062760A CN111164800A CN 111164800 A CN111164800 A CN 111164800A CN 201880062760 A CN201880062760 A CN 201880062760A CN 111164800 A CN111164800 A CN 111164800A
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China
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intermediate layer
active material
positive electrode
plate
insulating particles
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CN201880062760.1A
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田边森人
辻田幸平
大杉勇太
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GS Yuasa International Ltd
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GS Yuasa International Ltd
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/22—Electrodes
    • H01G11/26—Electrodes characterised by their structure, e.g. multi-layered, porosity or surface features
    • H01G11/28—Electrodes characterised by their structure, e.g. multi-layered, porosity or surface features arranged or disposed on a current collector; Layers or phases between electrodes and current collectors, e.g. adhesives
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H01M4/0402—Methods of deposition of the material
    • H01M4/0404—Methods of deposition of the material by coating on electrode collectors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/139—Processes of manufacture
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/624—Electric conductive fillers
    • H01M4/625—Carbon or graphite
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/661—Metal or alloys, e.g. alloy coatings
    • H01M4/662—Alloys
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/663—Selection of materials containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/665—Composites
    • H01M4/667—Composites in the form of layers, e.g. coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2220/00—Batteries for particular applications
    • H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/60—Other road transportation technologies with climate change mitigation effect
    • Y02T10/70—Energy storage systems for electromobility, e.g. batteries

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  • Chemical & Material Sciences (AREA)
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  • Power Engineering (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Electric Double-Layer Capacitors Or The Like (AREA)
  • Secondary Cells (AREA)

Abstract

An electrode plate includes a current collector, an intermediate layer laminated on the current collector, and an active material layer laminated on the intermediate layer. The intermediate layer contains conductive particles and insulating particles. At least a part of the edge of the intermediate layer is not covered with the active material layer. The mass content of the insulating particles in the region of the intermediate layer not covered with the active material layer is higher than the mass content of the insulating particles in the region covered with the active material layer.

Description

Electrode plate, electrode assembly and energy storage device
Technical Field
The invention relates to a polar plate, an electrode assembly and an energy storage device.
Background
Chargeable and dischargeable energy storage devices (secondary batteries) are used for various devices including mobile phones and electric vehicles. In recent years, with the increasing demand for high power and high performance of these devices, there is a demand for energy storage devices that are smaller and have a larger capacitance (larger energy density).
An energy storage device including an electrode assembly formed by alternately laminating positive electrode plates (positive electrode plates) including a current collector and a positive electrode active material layer formed on a surface of the current collector and negative electrode plates (negative electrode plates) including a current collector and a negative electrode active material layer formed on a surface of the current collector with an electrically insulating separator interposed therebetween is widely used. In such an energy storage device, thinning the spacer effectively increases the capacitance per unit volume of the device. Therefore, an energy storage device including a spacer formed of a porous resin film is put to practical use.
In an energy storage device including a separator formed of a resin film, a temperature increase of an electrode assembly, which does not occur in normal use but is caused by some factors, is likely to cause the separator to shrink by heat, thereby bringing a positive electrode plate into direct contact with a negative electrode plate. The contact of the collector of the electrode plate with the counter electrode plate (collector or active material layer) makes the electric resistance even smaller than that when the active material layers are in contact with each other, and thus a very large short-circuit current may flow to cause excessive heat generation. The electrode plate generally has a tab for connecting itself to an external terminal, the tab being formed by partially extending a current collector in a band shape such that the current collector protrudes from the active material layer. Therefore, the tab is highly likely to come into contact with the counter electrode plate when the temperature rises.
The electrode plate sometimes includes a so-called intermediate layer to improve adhesion between the collector and the active material layer. It is proposed to extend the intermediate layer to a region of the current collector where the active material layer is not laminated (for example, a tab) in order to prevent the current collector from directly contacting the counter electrode. The collector is in contact with the opposite electrode plate with the intermediate layer interposed therebetween, which causes an increase in short-circuit resistance (see, for example, JP- ｃA-2014-.
Documents of the prior art
Patent document
Patent document 1: JP-A-2014-75335
Disclosure of Invention
Problems to be solved by the invention
As described in the above patent documents, when the effect of suppressing the short-circuit current by the resistance of the intermediate layer is increased, it is necessary to increase the resistance of the intermediate layer, and the increase in the resistance of the intermediate layer also increases the resistance between the collector and the active material layer. Therefore, in the structure described in the above-mentioned patent document, an increase in the effect of suppressing the short-circuit current increases the internal loss caused by the resistance of the intermediate layer, so that the energy efficiency of the energy storage device may be reduced.
Under the above circumstances, an object of the present invention is to provide an electrode plate, an electrode assembly, and an energy storage device having a great effect of suppressing a short-circuit current between the electrode plate and an opposite electrode plate.
Means for solving the problems
A plate according to an aspect of the present invention, which is manufactured to solve the problem, includes a current collector, an intermediate layer laminated on the current collector, and an active material layer laminated on the intermediate layer, wherein the intermediate layer contains conductive particles and insulating particles, wherein at least a part of an end edge of the intermediate layer is not covered with the active material layer, and wherein a mass content of the insulating particles in a region of the intermediate layer not covered with the active material layer is higher than a mass content of the insulating particles in a region covered with the active material layer.
THE ADVANTAGES OF THE PRESENT INVENTION
The plate according to an aspect of the present invention has a great effect of suppressing a short-circuit current between the plate and the opposite plate.
Drawings
Fig. 1 is a schematic exploded perspective view of an energy storage device according to one embodiment of the invention.
Fig. 2 is a schematic cross-sectional view of an electrode assembly of the energy storage device of fig. 1.
Fig. 3 is a schematic top view of a positive electrode plate of the electrode assembly in fig. 2.
Fig. 4 is a schematic partially enlarged sectional view of the positive electrode plate in fig. 3.
FIG. 5 is a photograph illustrating an example according to one embodiment of the present invention.
Detailed Description
A plate according to an aspect of the present invention includes a current collector, an intermediate layer laminated on the current collector, and an active material layer laminated on the intermediate layer, the intermediate layer containing conductive particles and insulating particles, the intermediate layer having no active material layer laminated on at least a part of an end edge thereof, and the intermediate layer having a higher insulating particle mass content in a region on which an active material is not laminated than in a region on which an active material layer is laminated.
In this electrode plate, the intermediate layer laminated between the current collector and the active material layer has a higher content by mass of insulating particles in a region on which the active material layer is not laminated than in a region on which the active material layer is laminated, and therefore the intermediate layer has a larger resistance in the region on which the active material layer is not laminated than in the region on which the active material layer is laminated. Therefore, the electrode plate does not increase the internal resistance of an energy storage device formed using the electrode plate, but increases the short-circuit resistance during contact between the electrode plates, thereby being able to effectively suppress a short-circuit current.
In the plate, preferably, the conductive particles are a carbon material, and the insulating particles are alumina. This structure is considered to easily increase the difference in dispersibility between the conductive particles and the insulating particles in the coating solution for forming the intermediate layer by coating and drying. This makes it easy to increase the mass content of the insulating particles in the end edges of the intermediate layer, thereby making it easy to produce the plate.
In the electrode plate, the intermediate layer preferably further contains an aggregation inhibitor for regulating aggregation of the insulating particles. This structure enables the insulating particles to be suitably dispersed in a coating solution for forming the intermediate layer by coating and drying. This makes it easy to increase the mass content of the insulating particles in the end edges of the intermediate layer, thereby making it easy to produce the electrode plate.
An electrode assembly according to another aspect of the present invention includes the electrode plate, an opposite electrode plate opposite to the electrode plate and having a polarity different from that of the electrode plate, and a separator interposed between the electrode plate and the opposite electrode plate. The electrode assembly includes electrode plates having a high mass content of insulating particles in regions on which active materials are not stacked, thereby being capable of effectively suppressing short-circuit current during contact between the electrode plates and the opposite electrode plate.
An energy storage device according to another aspect of the present invention includes the electrode assembly and a case for accommodating the electrode assembly. The energy storage device includes the electrode assembly, so that a short-circuit current during contact between the electrode plate and the opposite electrode plate can be effectively suppressed.
Hereinafter, embodiments of the present invention are described in detail with reference to the accompanying drawings as appropriate.
Fig. 1 shows the structure of an energy storage device according to an embodiment of the present invention. The energy storage device includes an electrode assembly 1 and a case 2 for accommodating the electrode assembly 1. The case 2 is sealed with the electrode assembly 1 and the electrolyte. The electrode assembly 1 itself represents one embodiment of a laminated electrode assembly according to the present invention.
As shown in fig. 2, the electrode assembly 1 includes a plurality of positive electrode plates 3, a plurality of negative electrode plates 4, and a plurality of separators 5 interposed between the positive electrode plates 3 and the negative electrode plates 4, respectively, wherein the plurality of negative electrode plates 4 are opposed to the positive electrode plates 3 as opposed electrode plates which are alternately laminated so as to be opposed to the positive electrode plates and have a polarity different from that of the positive electrode plates. The positive plate 3 itself represents one embodiment of a plate according to the invention.
As shown in fig. 3 and 4, the positive electrode plate 3 includes a positive electrode collector 6, an intermediate layer 7 laminated on both surfaces of the positive electrode collector 6, and a positive electrode active material layer 8 laminated on a surface of the intermediate layer 7 opposite to the positive electrode collector 6.
The positive electrode current collector 6 includes: a rectangular active material region in plan view on which a positive electrode active material layer 8 is laminated; and a positive electrode tab 9 extending from the active material region in a band shape with a small width.
A material used as the positive electrode collector 6 is a metal such as aluminum, iron, and nickel, or an alloy thereof. Among these materials, aluminum and aluminum alloys are more preferable in order to balance between high conductivity and cost. Examples of the morphology of the positive electrode collector 6 include foil and deposited film, and foil is preferable in terms of cost. That is, aluminum foil is preferably used as the positive electrode current collector 6. Examples of aluminum and aluminum alloys include a1085P and a3003P specified in JIS H4000 (2014).
The lower limit of the average thickness of the positive electrode current collector 6 is preferably5μ m, more preferably 10 μm. On the other hand, the upper limit of the average thickness of the positive electrode current collector 6 is preferably 40 μm, and more preferably 20 μm. When the average thickness of the positive electrode current collector 6 is set to the lower limit or more, the positive electrode current collector 6 can be made to have sufficient strength. In the case where the average thickness of the positive electrode current collector 6 is set to the above upper limit or less, the energy density of the electrode assembly 1 can be increased.
The intermediate layer 7 is interposed between the positive electrode current collector 6 and the positive electrode active material layer 8 to improve the adhesion strength of the positive electrode active material layer 8 to the positive electrode current collector 6. The intermediate layer 7 has conductivity to electrically connect the positive electrode current collector 6 to the positive electrode active material layer 8.
When the separator 5 thermally contracts due to overheating of the energy storage device, which does not occur in normal use but is caused by some factors, the intermediate layer 7 prevents the positive electrode collector 6 from directly contacting the negative electrode plate 4, thereby suppressing the short-circuit current by the resistance of the intermediate layer 7. Therefore, the intermediate layer 7 is preferably laminated over the entire region of the positive electrode collector 6 facing the negative electrode plate 4.
The intermediate layer 7 contains a plurality of conductive particles, a plurality of insulating particles, and a binder for these particles. The intermediate layer 7 preferably further contains an aggregation inhibitor for regulating aggregation of the insulating particles. The intermediate layer 7 may also contain additives such as thickeners or flame retardants.
The intermediate layer 7 has no positive electrode active material layer 8 laminated on at least a part of its edge, and particularly has no positive electrode active material layer 8 laminated on the part of the positive electrode tab 9, and the part or the part is exposed to face the negative electrode plate 4. The intermediate layer 7 has a higher mass content of insulating particles in the exposed region on which the positive electrode active material layer 8 is not stacked than in the stacked region on which the positive electrode active material layer 8 is stacked.
The intermediate layer 7 may be formed by coating the positive electrode current collector 6 with a coating solution prepared by dispersing conductive particles and insulating particles in a binder solution obtained by dissolving a binder in a solvent and drying the coating solution. It is considered that appropriate adjustment of the aggregation property of the insulating particles in the coating solution can form an exposed region having a high mass content of the insulating particles at the outer edge portion of the coating region during drying by the coffee ring effect. The "coffee ring effect" refers to the following phenomenon: the evaporation amount of the dispersion medium is increased in the outer edge of the coating region to concentrate and aggregate the dispersoid in the outer edge portion of the coating region, so that the dispersoid is concentratedly left in the outer edge portion after drying.
The lower limit of the surface resistance in the laminated region of the intermediate layer 7 is preferably 0.03 m.OMEGA/□, more preferably 0.05 m.OMEGA/□. On the other hand, the upper limit of the surface resistance in the laminated region of the intermediate layer 7 is preferably 40m Ω/□, and more preferably 20m Ω/□. When the surface resistance in the laminated region of the intermediate layer 7 is set to the lower limit or more, the surface resistance of the exposed region can be sufficiently increased. When the surface resistance in the laminated region of the intermediate layer 7 is set to the upper limit or less, the loss due to the internal resistance of the energy storage device can be sufficiently reduced. The surface resistance of the laminated region of the intermediate layer 7 was measured by a four-terminal method using MCP-TESTER LORESTA-FP (manufactured by Mitsubishi petrochemical Co., Ltd.).
The lower limit of the surface resistance in the exposed region of the intermediate layer 7 is preferably 500 m.OMEGA./□, more preferably 1 Ω/□. On the other hand, the upper limit of the surface resistance in the exposed region of the intermediate layer 7 is preferably 200 Ω/□, and more preferably 100 Ω/□. When the surface resistance of the exposed region of the intermediate layer 7 is set to the lower limit or more, the short-circuit current can be sufficiently suppressed when the exposed region of the intermediate layer 7 is in contact with the negative electrode plate 4. When the surface resistance in the exposed region of the intermediate layer 7 is set to the upper limit or less, the surface resistance in the laminated region of the intermediate layer 7 can be sufficiently reduced. The surface resistance of the exposed region of the intermediate layer 7 was measured by a four-terminal method using MCP-TESTER LORESTA-FP (manufactured by Mitsubishi petrochemical Co., Ltd.).
The lower limit of the average thickness of the intermediate layer 7 is preferably 0.5 μm, more preferably 1 μm. On the other hand, the upper limit of the average thickness of the intermediate layer 7 is preferably 20 μm, and more preferably 5 μm. When the average thickness of the intermediate layer 7 is set to the lower limit or more, the mass content of the insulating particles in the region where the positive electrode active material layer 8 is not stacked can be easily increased, and therefore the productivity of the positive electrode plate 3 can be improved. In the case where the average thickness of the intermediate layer 7 is set to the upper limit or less, the thickness of the positive electrode plate 3 can be reduced, and therefore the energy density of the energy storage device can be increased.
The conductive particles contained in the intermediate layer 7 ensure conductivity between the positive electrode current collector 6 and the positive electrode active material layer 8.
Examples of the conductive particles in the intermediate layer 7 include: carbon materials such as graphite, furnace black, acetylene black, and ketjen black; metals such as iron, nickel, copper, aluminum, gold, and silver; and a conductive ceramic. Among these materials, a carbon material is particularly suitable in terms of easily distinguishing the behavior of the conductive particles in the dispersion medium from the behavior of the insulating particles described later. Examples of carbon materials used as the conductive particles include carbon black such as furnace black, acetylene black, and ketjen black, and graphite.
The lower limit of the average particle diameter of the conductive particles in the intermediate layer 7 is preferably 0.001 μm, and more preferably 0.003 μm. On the other hand, the upper limit of the average particle diameter of the conductive particles in the intermediate layer 7 is preferably 1 μm, and more preferably 0.5 μm. In the case where the average particle diameter of the conductive particles in the intermediate layer 7 is set to the above-described lower limit or more, the conductive particles can be easily dispersed in the coating solution forming the intermediate layer 7, thereby giving a constant resistance in the laminated region. In the case where the average particle diameter of the conductive particles in the intermediate layer 7 is set to the upper limit or less, the intermediate layer 7 having a uniform thickness can be formed. The "average particle diameter" refers to an average value of equivalent circle diameters of particles measured in a microscopic observation image according to Z8827-1 (2008).
The lower limit of the content of the conductive particles in the entire intermediate layer 7 is preferably 3% by mass, and more preferably 5% by mass. On the other hand, the upper limit of the content of the conductive particles in the entire intermediate layer 7 is preferably 40% by mass, and more preferably 30% by mass. In the case where the content of the conductive particles in the entire intermediate layer 7 is set to the above-described lower limit or more, the conductivity of the intermediate layer 7 can be ensured. In the case where the content ratio of the conductive particles in the entire intermediate layer 7 is set to the upper limit or less, the resistance of the exposed region of the intermediate layer 7 can be sufficiently increased.
The insulating particles contained in the intermediate layer 7 regulate the conductivity of the intermediate layer 7 to increase the resistance particularly in the exposed region of the intermediate layer 7, thereby suppressing short-circuit current when the separator 5 contracts to bring the positive electrode plate 3 into contact with the negative electrode plate 4.
Examples of the insulating particles in the intermediate layer 7 include zinc oxide, titanium oxide, iron oxide, aluminum oxide, boron nitride, aluminum hydroxide, silicon oxide, and polyolefins (PE, PP, and PTFE). Among these materials, a metal oxide is suitable in terms of easily distinguishing the behavior of the insulating particles in the dispersion medium from the behavior of the aforementioned conductive particles, and among the metal oxides, alumina is particularly suitably used.
The lower limit of the average particle diameter of the insulating particles in the intermediate layer 7 is preferably 0.01 μm, and more preferably 0.10 μm. On the other hand, the upper limit of the average particle diameter of the insulating particles in the intermediate layer 7 is preferably 10 μm, and more preferably 5 μm. In the case where the average particle diameter of the insulating particles in the intermediate layer 7 is set to the above-described lower limit or more, the insulating particles can be uniformly dispersed in the laminated region of the intermediate layer 7. In the case where the average particle diameter of the insulating particles in the intermediate layer 7 is set to the upper limit or less, the mass content of the insulating particles in the outer edge portion can be increased by the coffee ring effect, and therefore the electric resistance in the exposed region of the intermediate layer 7 can be sufficiently increased. When the particle diameter is small, the coffee ring effect tends to increase, and therefore, the average particle diameter of the insulating particles in the intermediate layer 7 is more preferably smaller than the average particle diameter of the conductive particles.
The lower limit of the content of the insulating particles in the entire intermediate layer 7 is preferably 40% by mass, and more preferably 50% by mass. On the other hand, the upper limit of the content of the insulating particles in the entire intermediate layer 7 is preferably 90 mass%, and more preferably 85 mass%. When the content of the insulating particles in the entire intermediate layer 7 is set to the lower limit or more, the resistance of the exposed region of the intermediate layer 7 can be sufficiently increased. In the case where the content ratio of the insulating particles in the entire intermediate layer 7 is set to the upper limit or less, the content ratios of the conductive particles and the binder can be secured, and thus the adhesiveness and the conductivity in the laminated region can be secured.
The binder contained in the intermediate layer 7 makes connection between the conductive particles and the insulating particles, and the adhesiveness of the intermediate layer 7 to the positive electrode collector 6 and the positive electrode active material layer 8 is applied.
As the binder contained in the intermediate layer 7, resins such as polyvinylidene fluoride, styrene-butadiene rubber, chitosan, polyethylene, polypropylene, polytetrafluoroethylene, and polyacrylic acid can be used.
The lower limit of the content of the binder in the entire intermediate layer 7 is preferably 5% by mass, and more preferably 10% by mass. On the other hand, the upper limit of the content of the binder in the entire intermediate layer 7 is preferably 60% by mass, and more preferably 50% by mass. In the case where the content of the binder in the entire intermediate layer 7 is set to the above-described lower limit or more, the strength of the intermediate layer 7 can be ensured. In the case where the content ratio of the binder in the entire intermediate layer 7 is set to the upper limit or less described above, conductivity can be obtained in the laminated region of the intermediate layer 7.
The aggregation inhibitor that may be contained in the intermediate layer 7 has an effect of regulating aggregation of the insulating particles, and due to the coffee ring effect, a region in which the content rate of the insulating particles is high can be formed in the outer edge portion of the intermediate layer 7. For example, since the effect of the aggregation inhibitor can be enhanced by mixing the insulating particles and the aggregation inhibitor in advance to attach the aggregation inhibitor to the surfaces of the insulating particles, a region with a high content of the insulating particles can be formed relatively easily in the outer edge portion of the intermediate layer 7.
As the aggregation inhibitor that may be contained in the intermediate layer 7, various surfactants such as an anionic surfactant, a cationic surfactant, a bipolar surfactant, a nonionic surfactant, and a polymer surfactant may be used. Among these surfactants, particularly suitably used are polymer surfactants capable of suitably suppressing aggregation of insulating particles.
The lower limit of the content of the aggregation inhibitor in the entire intermediate layer 7 is preferably 0.5% by mass, and more preferably 1% by mass. On the other hand, the upper limit of the content of the aggregation inhibitor in the entire intermediate layer 7 is preferably 5% by mass, and more preferably 4% by mass. When the content of the aggregation inhibitor is set within the above range, the aggregation property of the insulating particles can be appropriately adjusted.
As a dispersion medium of the coating solution for forming the intermediate layer 7, any substance capable of dissolving the binder can be used. Examples of the dispersion medium include organic solvents such as N-methyl-2-pyrrolidone and toluene, and water, and these dispersion media may be used alone or in a mixed plurality.
The lower limit of the solid content in the coating solution for forming the intermediate layer 7 is preferably 10% by mass, and more preferably 15% by mass. On the other hand, the upper limit of the solid content in the coating solution for forming the intermediate layer 7 is preferably 30% by mass, and more preferably 25% by mass. When the solid content ratio in the coating solution for forming the intermediate layer 7 is set to the lower limit or more, the thickness of the intermediate layer 7 can be secured, and the resistance in the laminated region can be appropriately adjusted. In the case where the content of the solid component in the coating solution for forming the intermediate layer 7 is set to the above-described upper limit or less, the content of the insulating particles in the exposed region formed by the coffee ring during drying of the coating solution can be relatively increased.
The lower limit of the viscosity of the coating solution for forming the intermediate layer 7 is preferably 10Pa · s, and more preferably 100Pa · s. On the other hand, the upper limit of the viscosity of the coating solution for forming the intermediate layer 7 is preferably 10000Pa · s, and more preferably 1000Pa · s. In the case where the viscosity of the coating solution for forming the intermediate layer 7 is set to the above-described lower limit or more, the thickness of the intermediate layer 7 can be secured, so that the resistance in the laminated region can be appropriately adjusted. When the viscosity of the coating solution for forming the intermediate layer 7 is set to the upper limit or less, uniform coating can be performed, and finally the intermediate layer 7 having a uniform thickness can be formed. The viscosity of the coating solution is a value measured using a B-type viscometer. Specifically, the viscosity is a value measured after 3 minutes using the same machine as TVB-15 type (manufactured by TOKI SANGYO Co., Ltd.) using a No. 3 rotor at a rotation speed of 12 rpm.
The upper limit of the drying time (time required to reduce the content of the dispersion medium to 10% by mass or less) for drying the coating solution for forming the intermediate layer 7 is preferably 20 minutes, and more preferably 10 minutes. When the drying time for drying the coating solution for forming the intermediate layer 7 is set to the upper limit or less, the production efficiency of the positive electrode plate 3 can be improved.
The aggregation inhibitor is likely to adhere to both the conductive particles and the insulating particles. Therefore, it is considered that the aggregation property of the insulating particles can be appropriately adjusted by previously mixing the aggregation inhibitor with one of the conductive particles and the insulating particles in accordance with the content ratio of the aggregation inhibitor to preferentially adhere the aggregation inhibitor to the surface of one of the conductive particles and the insulating particles.
The positive electrode active material layer 8 is formed of a so-called positive electrode mixture containing a positive electrode active material. The positive electrode mixture for forming the positive electrode active material layer 8 contains optional components such as a conductive agent, a binder, or a thickener as necessary.
Examples of the positive electrode active material include a composite oxide represented by LixMOy (M represents at least one transition metal) (e.g., LixCoO2, LixNiO2, LixMn2O4, LixMnO3, LixNi α Co (1- α) O2, LixNi α Mn β Co (1- α - β) O2, and LixNi α Mn (2- α) O4), and a polyanionic compound represented by liwmmex (xoy) z (Me represents at least one transition metal, and X represents, for example, P, Si, B, or V) (e.g., LiFePO4, LiMnPO4, ipo4, LiCoPO4, Li3V2(PO4)3, Li2MnSiO4, and Li2CoPO 4F.) other elements or anionic species may be used instead of part of these active elements or polyanionic species as a positive electrode active material or a mixture of these positive electrode active materials, and these active material may be used alone or as a positive electrode active material.
The lower limit of the content of the positive electrode active material in the positive electrode active material layer 8 is preferably 50 mass%, more preferably 70 mass%, and still more preferably 80 mass%. On the other hand, the upper limit of the content of the positive electrode active material is preferably 99 mass%, and more preferably 94 mass%. When the content of the positive electrode active material is set to the lower limit or more, the energy density of the electrode assembly 1 can be increased. When the content of the positive electrode active material is set to the upper limit or less, the strength of the positive electrode active material layer 8 can be ensured.
The conductive agent is not particularly limited as long as it is a conductive material that does not adversely affect the performance of the battery. Examples of such a conductive agent include: natural or artificial graphite; carbon black such as furnace black, acetylene black and ketjen black; a metal; and a conductive ceramic. Examples of the shape of the conductive agent include powder and fiber.
The lower limit of the content of the conductive agent in the positive electrode active material layer 8 is preferably 0.1 mass%, and more preferably 0.5 mass%. On the other hand, the upper limit of the content of the conductive agent is preferably 10% by mass, and more preferably 5% by mass. In the case where the content ratio of the conductive agent is set within the above range, the energy density of the electrode assembly 1 can be increased, so that the energy density of the energy storage device can be increased.
Examples of the binder include thermoplastic resins such as fluororesins (e.g., polytetrafluoroethylene and polyvinylidene fluoride), polyethylene, polypropylene, and polyimide, elastomers such as ethylene-propylene-diene rubber (EPDM), sulfonated EPDM, styrene-butadiene rubber, and fluororubber, and polysaccharide polymers.
The lower limit of the content of the binder in the positive electrode active material layer 8 is preferably 1% by mass, and more preferably 2% by mass. On the other hand, the upper limit of the content of the binder is preferably 10% by mass, and more preferably 5% by mass. When the content of the binder is set within the above range, the positive electrode active material can be stably held.
Examples of thickeners include polysaccharide polymers such as carboxymethyl cellulose and methyl cellulose. When the thickener has a functional group reactive with lithium, it is preferable to deactivate the functional group in advance, for example, by methylation.
The lower limit of the average thickness of the positive electrode active material layer 8 is preferably 10 μm, and more preferably 20 μm. On the other hand, the upper limit of the average thickness of the positive electrode active material layer 8 is preferably 200 μm, and more preferably 100 μm. In the case where the average thickness of the positive electrode active material layer 8 is set to the above-described lower limit or more, the positive electrode reaction can be sufficiently activated. In the case where the average thickness of the positive electrode active material layer 8 is set to the upper limit or less, the energy density of the electrode assembly 1 can be increased, and thus the energy density of the energy storage device can be increased.
The negative electrode plate 4 includes a conductive foil-or sheet-shaped negative electrode collector 10 and a negative electrode active material layer 11 laminated on a surface of the negative electrode collector 10. Specifically, the negative electrode plate 4 includes an active material region of a rectangular shape in plan view on which an active material layer is laminated on the surface of the negative electrode collector 10, and includes a negative electrode tab 12 extending from the active material region in a belt shape having a width smaller than the width of the active material region in the same direction as the positive electrode tab 9 with a gap between the negative electrode tab and the positive electrode tab 9.
The negative electrode collector 10 of the negative electrode plate 4 may have the same structure as the positive electrode collector 6 described above. However, the material of the negative electrode collector is preferably copper or a copper alloy. That is, the negative electrode collector 10 of the negative electrode plate 4 is preferably a copper foil. Examples of the copper foil include rolled copper foil and electrolytic copper foil.
The anode active material layer 11 is formed of a so-called anode plate mixture containing an anode active material. The negative electrode plate mixture for forming the negative electrode active material layer 11 contains optional components such as a conductive agent, a binder, a thickener, or a filler as needed. Optional components such as a conductive agent, a binder, a thickener, or a filler may use the same components as those in the positive electrode active material layer 8.
Suitable as the negative electrode active material are materials capable of storing and releasing lithium ions. Specific examples of the negative electrode active material include: metals such as lithium and lithium alloys; a metal oxide; a polyphosphoric acid compound; and carbon materials such as graphite, amorphous carbon (graphitizable carbon or non-graphitizable carbon).
The lower limit of the content of the negative electrode active material in the negative electrode active material layer 11 is preferably 60 mass%, more preferably 80 mass%, and still more preferably 90 mass%. On the other hand, the upper limit of the content of the negative electrode active material is preferably 99 mass%, and more preferably 98 mass%. In the case where the content ratio of the anode active material is set within the above range, the energy density of the electrode assembly 1 can be increased, so that the energy density of the energy storage device can be increased.
The lower limit of the content of the binder in the negative electrode active material layer 11 is preferably 1% by mass, and more preferably 5% by mass. On the other hand, the upper limit of the content of the binder is preferably 20% by mass, and more preferably 15% by mass. When the content of the binder is set within the above range, the negative electrode active material can be stably held.
The lower limit of the average thickness of the anode active material layer 11 is preferably 10 μm, and more preferably 20 μm. On the other hand, the upper limit of the average thickness of the anode active material layer 11 is preferably 200 μm, and more preferably 100 μm. In the case where the average thickness of the anode active material layer 11 is set to the above-described lower limit or more, the anode reaction can be sufficiently activated. In the case where the average thickness of the anode active material layer 11 is set to the upper limit or less, the energy density of the electrode assembly 1 can be increased, so that the energy density of the energy storage device can be increased.
The separator 5 is interposed between the positive electrode plate 3 and the negative electrode plate 4 to prevent the positive electrode plate 3 and the negative electrode plate 4 from directly contacting, and is impregnated with an electrolyte inside, so that electric charges can be transported between the positive electrode plate 3 and the negative electrode plate 4 via ions.
The spacer 5 may be formed of a porous resin film. The separator 5 may include an oxidation resistant layer or a heat resistant layer on at least one surface (preferably, a surface opposite to the positive electrode plate 3) of the porous resin film, and may include an adhesive layer as an outermost layer for bonding the separator 5 to the positive electrode plate 3 or the negative electrode plate 4.
As the main component of the porous resin film used to form the spacer 5, polyethylene, polypropylene, ethylene-vinyl acetate copolymer, and ethylene-methyl acrylate copolymer can be used, for example. Of these components, the main components suitable for use as the porous resin film for forming the separator 5 are polyethylene and polypropylene excellent in resistance to electrolytic solution and durability. "major component" means the component having the highest mass content.
The lower limit of the average thickness of the porous resin film for forming the spacer 5 is preferably 5 μm, and more preferably 10 μm. On the other hand, the upper limit of the average thickness of the porous resin film for forming the spacer 5 is preferably 30 μm, and more preferably 20 μm. When the average thickness of the porous resin film for forming the spacer 5 is set to the lower limit or more, the strength of the spacer 5 can be ensured. When the average thickness of the porous resin film for forming the separator 5 is set to the upper limit or less, the energy density of the electrode assembly 1 can be increased, and the energy density of the energy storage device can be increased.
The oxidation resistant layer or heat resistant layer of the spacer 5 is a layer provided for suppressing the porous resin film for forming the spacer 5 from being oxidized and deteriorated, and includes many inorganic particles and a binder connecting between the inorganic particles.
Examples of the main component of the inorganic particle include alumina, silica, zirconia, titania, magnesia, and boehmite. Among these components, aluminum, silica and titanium oxide are particularly preferable as the main components of the inorganic particles in the antioxidation layer or the heat-resistant layer.
The lower limit of the average particle diameter of the inorganic particles in the antioxidation layer or the heat-resistant layer is preferably 1nm, and more preferably 7 nm. On the other hand, the upper limit of the average particle diameter of the inorganic particles is preferably 5 μm, and more preferably 1 μm. In the case where the average particle diameter of the inorganic particles is set to the above-described lower limit or more, the proportion of the binder in the antioxidation layer or the heat-resistant layer can be reduced, so that the heat resistance of the antioxidation layer or the heat-resistant layer can be improved. In the case where the average particle diameter of the inorganic particles is set to the upper limit or less, a uniform antioxidation layer or heat-resistant layer can be formed.
The lower limit of the average thickness of the antioxidation layer or the heat-resistant layer is preferably 2 μm, more preferably 4 μm. On the other hand, the upper limit of the average thickness of the antioxidation layer or the heat-resistant layer is preferably 6 μm, and more preferably 5 μm. In the case where the average thickness of the antioxidation layer or the heat-resistant layer is set to the above-described lower limit or more, the strength of the antioxidation layer or the heat-resistant layer can be ensured. In the case where the average thickness of the antioxidation layer or the heat-resistant layer is set to the above-described upper limit or less, the energy density of the electrode assembly 1 can be increased, so that the energy density of the energy storage device can be increased.
As the electrolytic solution, an organic electrolytic solution obtained by dissolving the supporting electrolytic solution in an organic solvent is used. A lithium salt is suitably used as the supporting electrolyte. The lithium salt is not particularly limited, and examples thereof include LiPF6, LiAsF6, LiBF4, LiSbF6, LiAlCl4, and LiClO 4. Among these lithium salts, LiPF6, LiClO4, and CF3SO3Li, which are easily soluble in organic solvents and exhibit a high dissociation degree, are particularly preferred.
The organic solvent used in the electrolytic solution is not particularly limited as long as it can dissolve the supporting electrolytic solution, and may be used alone or in combination of a plurality thereof, for example, dimethyl carbonate, ethylene carbonate, diethyl carbonate, propylene carbonate, and butylene carbonate. Among these organic solvents, carbonates having a high dielectric constant and having a wide stable potential region are particularly suitable for use.
The case 2 is a sealed case that houses the electrode assembly 1 and seals an electrolyte therein.
The material of the case 2 may be, for example, resin as long as it has sealability capable of sealing the electrolyte and has strength capable of protecting the electrode assembly 1. However, metal is suitably used as the material. In other words, the housing 2 may be, for example, a bag or the like formed of, for example, a laminated film and having flexibility. However, as the case, a hard metal case capable of more reliably protecting the electrode assembly 1 is preferably used.
The housing 2 may be configured to include a housing main body 13 in a square cylindrical shape with a bottom and a plate-like cover 14 for sealing an opening of the housing main body 13. A positive external terminal 15 and a negative external terminal 16, which are electrically connected to the positive tab 9 of the positive electrode plate 3 and the negative tab 12 of the negative electrode plate 4, respectively, are provided on the cover 14. Specifically, the positive electrode external terminal 15 and the negative electrode external terminal 16 are provided to penetrate the cover 14.
In the case 2, energy storage devices are attached to the positive and negative external terminals 15 and 16, and the cover may further include positive and negative connection members 17 and 18 connected to the positive and negative tabs 9 and 12 of the electrode assembly 1, respectively.
< advantages >
The positive electrode plate 3 includes an intermediate layer 7, the intermediate layer 7 having a higher content of insulating particles in the exposed region than in the laminated region, so that the exposed region of the intermediate layer 7 having a high content of insulating particles and having a relatively large resistance is interposed between the positive electrode collector 6 and the negative electrode plate 4, thereby suppressing short-circuit current when the separator 5 thermally contracts due to overheating of the energy storage device, which does not occur in normal use, due to some factors. Further, the exposed region allows foreign matter to adhere thereto to prevent the foreign matter from entering between the electrode plates, so that, for example, short-circuiting due to the inclusion of foreign matter can be prevented.
[ other examples ]
The above embodiments do not limit the structure of the present invention. Therefore, the above-described embodiments allow the omission, replacement, or addition of constituent elements of each part in the embodiments based on the description of the present specification and the common technical knowledge, and those obtained by the omission, replacement, or addition are considered to be within the scope of the present invention.
The plate according to the invention may be a negative plate. That is, similar to the cathode plate according to the present invention, the anode plate may include an intermediate layer that is laminated between the anode current collector and the anode active material layer and has a higher content of insulating particles in a region on which the anode active material layer is not laminated than in a region on which the anode active material layer is laminated.
The present embodiment provides a plate including a tab. However, the plate may be a plate that does not include tabs. For example, when the intermediate layer and the active material layer are coated on the strip-shaped current collector, a region (uncoated region) where neither the intermediate layer nor the active material layer is coated may be formed at an end portion in the width direction of the strip shape to ensure electrical connection to the external terminal in the uncoated region.
Examples of the invention
Hereinafter, the present invention is described based on examples. However, the present invention is not limited to these examples.
(examples)
Alumina as an insulating particle and N-methyl-2-pyrrolidone were mixed at a mass ratio of 50:50, and a polymer surfactant as an aggregation inhibitor was added and mixed at 4 mass% with respect to the mass of alumina to prepare a preliminary coating solution having a solid content of about 50%. To the preliminary coating solution, acetylene black (conductive particles) and polyvinylidene fluoride (binder) were added and mixed at a mass ratio of alumina, acetylene black and polyvinylidene fluoride of 77:8:15 to obtain an actual coating solution. The actual coating solution was adjusted to have a solid content of 18%.
The actual coating solution was coated on a strip-shaped aluminum foil (current collector) with a doctor blade, and then dried in a constant temperature room at 80 ℃ for 20 minutes to obtain an aluminum foil of the present example. Fig. 5 shows a photograph of the aluminum foil obtained in the present example. In the intermediate layer, the central portion was black and the outer edge portions were white, indicating that the mass content of alumina in the contour edge portions was high.
In this example, a high-conductivity region (a region where the mass content of the insulating particles is low) and a high-resistance region (a region where the mass content of the insulating particles is high) can be formed by one-time application of the intermediate layer. That is, the high-conductivity region and the high-resistance region can be formed at the same time, and the present example can form the two regions more efficiently than the manner in which the two regions are formed separately.
INDUSTRIAL APPLICABILITY
The electrode plate, the electrode assembly and the energy storage device according to the present invention are particularly suitable for use as a power source for vehicles such as electric vehicles and plug-in hybrid electric vehicles (PHEVs). The energy storage device according to the invention may be suitable for industrial use such as energy storage systems (large energy storage systems and small energy storage systems for domestic use), for example distributed power systems incorporating natural energy sources such as sunlight or wind, railway power systems and Automatic Guided Vehicle (AGV) power systems.
Description of the reference numerals
1 electrode Assembly
2 casing
3 positive polar plate (Positive plate)
4 negative pole plate (opposite direction plate)
5 spacer
6 positive electrode current collector
7 intermediate layer
8 Positive electrode active material layer
9 positive pole ear
10 negative electrode collector
11 negative electrode active material layer
12 negative pole tab
13 casing body
14 cover
15 positive external terminal
16 negative electrode external terminal
17 Positive electrode connecting member
18 a negative electrode connecting member.

Claims (5)

1. A pole plate, comprising:
a current collector;
an intermediate layer laminated on the current collector; and
an active material layer laminated on the intermediate layer,
wherein the intermediate layer comprises conductive particles and insulating particles,
wherein at least a part of the edge of the intermediate layer is not covered with the active material layer, and
wherein a mass content of the insulating particles in a region of the intermediate layer not covered with the active material layer is higher than a mass content of the insulating particles in a region covered with the active material layer.
2. The plate as claimed in claim 1, wherein the conductive particles comprise a carbon material and the insulating particles comprise alumina.
3. The plate as claimed in claim 1 or 2, wherein the intermediate layer further comprises an aggregation inhibitor for regulating aggregation of the insulating particles.
4. An electrode assembly, comprising:
a plate as claimed in any of claims 1 to 3;
an opposite pole plate opposite to the pole plate and having a polarity different from that of the pole plate; and
a spacer interposed between the plate and the opposing plate.
5. An energy storage device, comprising:
the electrode assembly of claim 4; and
a case for accommodating the electrode assembly.
CN201880062760.1A 2017-11-29 2018-11-22 Electrode plate, electrode assembly and energy storage device Pending CN111164800A (en)

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